农业固废基水凝胶用于水体中重金属吸附的研究进展

侯文静; 何彩庆; 陈文清

doi:10.13801/j.cnki.fhclxb.20231213.002

农业固废基水凝胶用于水体中重金属吸附的研究进展

doi: 10.13801/j.cnki.fhclxb.20231213.002

四川大学　建筑与环境学院，成都 610065

详细信息

通讯作者:
陈文清，博士，教授，博士生导师，研究方向为环境功能材料研制及应用技术研究、富营养化水体及污染场地评估与生态修复　E-mail: chenwenqing@scu.edu.cn

中图分类号: TQ427.26；X703；TB332
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- 文章访问数: 327
- HTML全文浏览量: 205
- PDF下载量: 41
- 被引次数: 0
出版历程
- 收稿日期: 2023-10-16
- 修回日期: 2023-11-18
- 录用日期: 2023-12-04
- 网络出版日期: 2023-12-13
- 刊出日期: 2024-07-01

Adsorption of heavy metals by agricultural solid waste based hydrogel: A review

College of Architecture and Environment, Sichuan University, Chengdu 610065, China

摘要

摘要: 随着经济的快速发展，水中重金属离子污染对人类健康以及生态系统造成威胁。水凝胶以其良好的吸附性能、可再生性和低毒性在处理重金属离子方面具有很大的潜力。本文论述了近年来国内外以农业固体废弃物为原料制备水凝胶(纤维素基水凝胶、半纤维素基水凝胶、木质素基水凝胶等)吸附重金属的研究进展。同时，讨论了农业固废基水凝胶的合成，对重金属的吸附效果、吸附机制及分析方法，并列举了工业固废基和其他固废基水凝胶吸附重金属的效果，以期帮助研究者对农业固废基水凝胶吸附重金属的探究有更深刻的理解。
- 水凝胶复合材料 /
- 农业废弃物 /
- 重金属 /
- 吸附机制 /
- 水污染治理
Abstract: With the rapid development of economy, the pollution of heavy metal ions in water poses a threat to human health and ecosystem. Hydrogels have great potential in the treatment of heavy metal ions because of their good adsorption properties, renewability and low toxicity. This paper discusses the research progress in recent years on the preparation of hydrogels (cellulose-based hydrogels, hemicellulose-based hydrogels, lignin-based hydrogels, etc.) for the adsorption of heavy metals from agricultural solid wastes at home and abroad. The synthesis of agricultural solid waste based hydrogels, the adsorption effect, adsorption mechanism, and analytical methods for the removal of heavy metals are also discussed, and the effects of heavy metal adsorption by industrial solid waste based and other solid waste based hydrogels are enumerated. In order to help the researchers to have a deeper understanding of the investigation of heavy metal adsorption by agricultural solid waste based hydrogels.
- hydrogel composites /
- agricultural waste /
- heavy metals /
- adsorption mechanism /
- water pollution control

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图 1 农业固废基水凝胶用于水体中重金属吸附的示意图

Figure 1. Schematic diagram of agricultural solid waste-based hydrogel for heavy metal adsorption in water bodies

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图 2 农业固废基水凝胶合成示意图

Figure 2. Schematic synthesis of agricultural solid waste-based hydrogel

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图 3 农业固废基水凝胶吸附重金属的示意图

Figure 3. Schematic diagram of heavy metal adsorption on agricultural solid waste based hydrogel

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图 4 3种机制的吸附过程示意图

Figure 4. Schematic diagram of the adsorption process of the three mechanisms

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图 5 固废基水凝胶用于水体中重金属吸附的示意图

Figure 5. Schematic diagram of solid waste-based hydrogel for heavy metal adsorption in water bodies

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表 1 重金属对人类健康的危害

Table 1. Hazards of heavy metals to human health

Heavy metal	Harm to mankind
Pb	Accumulates in the bones, brain, kidneys and muscles of the body, leading to brain damage, mental retardation, anemia and cancer^[21]
Hg	Lung, kidney and chest pain, dyspnea injury^[22]
Cd	Cadmium ions pose a threat to many organs such as kidneys, lungs and liver^[23]
Cu	Leading to liver damage, insomnia and Wilson disease^[24]
Zn	Zinc not only irritates the skin, but also causes headache, dry cough, dizziness and other symptoms^[25]
Cr	Destroy human metabolism, stimulate skin and lung cancer^[26]
As	Skin damage and affect the nervous system of the human body^[27]
Ni	Dermatitis, nausea, chronic asthma, cough^[27]
Mn	Excessive manganese can cause dizziness and fatigue, mental retardation, and cause neurotransmitter disorders^[28]

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表 2 农业固废基水凝胶的制备及特点

Table 2. Synthesis and characterization of agricultural solid waste-based hydrogels

	Solid waste-based raw materials and other reagents	Method	Characteristic	Ref.
Cellulose base	Soybean residue cellulose, chitosan, polyvinyl alcohol, nano-Fe₃O₄	Freeze-thaw method	The increase of cellulose content is beneficial to improve the mechanical strength and swelling properties of the hydrogel.	[44]
	Licorice residue cellulose, crosslinker epichlorohydrin	Solution polymerization	The adsorption capacity, chemical stability, pore size distribution and mechanical properties of the hydrogel are improved by using epichlorohydrin as cross-linking agent.	[45]
	Bagasse cellulose, polyvinyl alcohol, crosslinker glutaraldehyde	Microwave assisted irradiation	Microwave assisted irradiation technology can save time and energy.	[46]
	Wheat straw cellulose, monomer acrylic acid and acrylamide, crosslinker N, N'-methylene-bis-acrylamide, initiator ammonium persulfate	Free radical graft copolymerization	Hydrogel has good thermal stability at temperature below 392℃.	[47]
	Poplar wood flour cellulose, 3-mercaptopropionic acid, L-cysteamine hydrochloride, initiator ammonium persulfate	Ultraviolet photoinitiation	The cellulose ester synthesized by esterification of anhydride with cellulose under homogeneous condition has higher reaction activity.	[48]
	Banana cellulose, chitosan, crosslinker epichlorohydrin	Solution polymerization	There are a large number of hydrophilic groups of hydroxyl and amino groups in the synthesized hydrogel, and the surface distributes irregular pore structure.	[49]
Lignin based	Wheat straw lignin, montmorillonite, monomer acrylic acid, crosslinker N, N'-methylene-bis-acrylamide, initiator K₂S₂O₈-Na₂SO₃	Solution polymerization	Montmorillonite is introduced into lignin nanocomposites to improve the adsorption and mechanical properties of lignin nanocomposites.	[50]
	Mulberry lignin, monomer acrylic acid, intercalation agent citric acid modified montmorillonite, crosslinker N, N'-methylene-bis-acrylamide, initiator (NH₄)S₂O₈	Graft intercalation method	When the amount of lignin is too high, the excess lignin produces too many cross-linking points, which affects the gel strength and hinders the cross-linking reaction.	[51]
	Rice husk lignin, chitosan, polyacrylamide	Free radical polymerization	Lignin and chitosan are mixed as the first network to provide active functional groups for the removal of heavy metals. As a malleable second network, polyacrylamide forms a stable structural hydrogel adsorbent.	[52]
Hemicellulose group	Corn kernel hemicellulose, monomers acrylic acid and N-isopropyl acrylamide, crosslinker N, N'-methylene-bis-acrylamide, photoinitiator benzoin dimethyl ether	Ultraviolet photoinitiation	Pb²⁺ solution pH in the range of 3.5-4.5 and elevated temperature favored the adsorption of hydrogels.	[53]
	Reed hemicellulose, monomer acrylic acid, crosslinker N, N, N', N'-tetramethylethylenediamine	Free radical polymerization	After 8 cycles of adsorption-desorption, the hydrogel still has high adsorption efficiency for metal ions.	[39]
	Xylan hemicellulose, carrageenan, initiator ammonium persulfate, polyvinylpyrrolidone	Microwave assisted irradiation	Compared with cellulose, xylan hemicellulose is amorphous and consists of branched chains of various sugars, which is easier to dissolve in common solvents.	[54]
Other types of agriculture	Citrus peel pectin, crosslinker calcium chloride, metal organic frame (MOF)	In-situ method	MOFs can interact with other components or adjust the properties of hydrogel matrix.	[55]
	Pomelo peel pectin, monomers acrylic acid and acrylamide, initiator ammonium persulfate, crosslinker N, N'-methylene-bis-acrylamide	Graft copolymerization	Microwave extraction-alcohol precipitation method for pectin extraction has the advantages of strong selectivity, short operation time, low solvent consumption and excellent quality of extracted pectin.	[56]
	Livestock bone powder, sodium alginate	Solution polymerization	Adsorption kinetics and adsorption isotherms indicate that adsorption is chemically and physically interactive.	[57]

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表 3 农业固废基水凝胶吸附重金属的优缺点

Table 3. Advantages and disadvantages of heavy metal adsorption on agricultural solid waste-based hydrogels

Common type	Common ground	Advantage	Disadvantage
Cellulose based hydrogel	Advantages: The raw materials are non-toxic, biodegradable and low cost; Make the hydrogel biocompatible, biodegradable and improve its adsorption performance. Disadvantages: Unhomogeneity of raw materials, structural complexity, and difficulty in obtaining pure substances, and poor mechanical strength of prepared hydrogels.	Contains hydroxyl, carboxyl and hydrogen bonding to improve the adsorption and mechanical properties of hydrogels.	Refractory; After several cycles of use, the morphology and mechanical properties of the hydrogel will change considerably, resulting in an unstable adsorption capacity.
Hemicellulose based hydrogel		Contains functional groups such as hydroxyl, acetyl and carboxyl groups; Good water solubility.	The mechanical strength of the prepared hemicellulose-based hydrogels is poor due to the small molecular weight of hemicellulose and low degree of polymerization.
Lignin based hydrogel		Hydroxyl and carbonyl groups can chelate with metal ions; Active site for chemical reactions.	The inhomogeneity and structural complexity of lignin and the difficulty of obtaining pure lignin；And when the amount of lignin is too high, excess lignin produces too many cross-linking points, which affects the gel strength and hinders the cross-linking reaction.
Other agricultural solid waste-based hydrogels		Pectin contains reactive groups such as carboxyl and hydroxyl groups.	Insoluble; Pectins from different sources have different gelling and adsorption capacities due to different sizes and chemical structures, and are less stable.

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表 4 农业固废基水凝胶对重金属的吸附性能总结

Table 4. Summary of adsorption properties of agricultural solid waste-based hydrogels for heavy metals

	Hydrogel	Target pollutant	Adsorption condition	Maximum adsorption capacity/(mg·g⁻¹)	Adsorption kinetic/ adsorption isotherm	Recycling rate	Ref.
Cellulose base	Soybean residue cellulose magnetic hydrogel	Cu(II)	pH=5.0	15.94	Pseudo-second-order/ Freundlich	4 times ＞80%	[44]
	Licorice residue cellulose hydrogel	Pb(II) Cr(III) Cu(II)	pH=5.0(Pb) t=120 min, pH=4.0(Cr)(Cu) t=60 min	591.8 458.3 121.4	Pseudo-second-order/ Langmuir	5 times ＞75%	[45]
	Bagasse carboxymethyl cellulose hydrogel	Cu(II)	pH=5.0	2.3	—	—	[46]
	Wheat straw cellulose hydrogel	Cu(II) Mn(II)	500 mg/L Co (Cu) 400 mg/L Co (Mn)	238.1 176.9	Pseudo-second-order	—	[47]
	Aspen cellulose methacrylate hydrogel	Pb(II) Hg(II)	Hydrogel dosage 0.2 g	148.44 112.55	Pseudo-second-order/ Langmuir	—	[48]
	Grapefruit peel cellulose-based hydrogel	Cu(II) Cr(VI) Cd(II)	Hydrogel dosage 10 g/L, pH=7.0, T=33℃, t=60 min, 10 mg/L Co	Removal rate 96.21%, 98.02%, 95.43%	—	—	[59]
	Banana fiber-chitosan hydrogel	Cu(II) Cd(II) Pb(II)	Hydrogel dosage 5 g/L, t=40 min	Removal rate 98.35%, 79.22%, 77.3%	Pseudo-second-order	—	[49]
Lignin base	Wheat straw lignin-montmorillonite hydrogel	Cu(II)	pH=6.5	74.35	Pseudo-second-order/ Freundlich	5 times ＞80%	[50]
Lignin base	Mulberry lignin hydrogel	Mn(II) Zn(II) Pb(II)	320 mg/L Co (Mn), 160 mg/L Co (Zn), 1000 mg/L Co (Pb), t =720 min	77.09 73.95 383.90	—	—	[51]
Hemicellulose based	Reed hemicellulose-based hydrogel	Pb(II) Cd(II) Zn(II)	200 mg/L Co, pH=5.5(Pb), pH=6.5(Cd)(Zn)	699 521 265	Pseudo-second-order/ Langmuir	—	[39]
Hemicellulose based	Yellow bamboo xylan hemicellulose-acrylic hydrogel	Pb(II) Cd(II) Zn(II)	t=60 min, pH=5.5(Pb), pH=6.5(Cd)(Zn)	859 495 274	Pseudo-second-order/ Langmuir	5 times ＞90%	[60]
Other categories	Metal-organic frame composite citrus peel gum hydrogel	Cr(VI) Pb(II)	pH=1(Cr), pH=5(Pb)	825.97 913.88	Pseudo-second-order/ Langmuir	8 times ＞85%	[55]
	Grapefruit peel pectin-based composite hydrogel	Cu(II)	pH=6.0	80.6	Pseudo-second-order/ Freundlich	4 times ＞90%	[61]
	Bone hydrogel of abandoned livestock and poultry in rural area	Cd(II)	pH=4.0, t=720 min	1010.19	Pseudo-second-order and intra-particle diffusion models/ Langmuir and Freundlich	3 times ＞90%	[57]
Notes: T—Temperature; t—Time.

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表 5 工业固废基水凝胶对重金属的吸附性能总结

Table 5. Summary of adsorption properties of industrial solid waste-based hydrogels for heavy metals

Hydrogel adsorption material	Target pollutant	Adsorption condition	Maximum adsorption capacity/(mg·g⁻¹)	Ref.
Red mud-sodium alginate hydrogel	Pb(II)	pH=6.0, T=25℃, t=900 min, 900 mg/L Co	454.54	[80]
Fly ash-hydroxyethyl cellulose-chitosan hydrogel	Cu(II)	100 mg/L Co	130.7	[81]
Modified fly ash-sodium alginate crosslinked acrylic hydrogel	Cu(II)	300 mg/L Co	131.09	[82]
Magnetic attapulgite/fly ash/polyacrylic acid hydrogel	Pb(II)	pH=5.0, 100 mg/L Co, t=24 h	38	[83]
Tobe mullite-starch hydrogel	Cd(II)	t=12 h, pH=5.21, T=25℃, hydrogel dosage 0.05 g	591.36	[84]

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